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Journal of the Physical Society of Japan

Observation of Two-Quantum Rotary Echoes in Multi-Level NMR System

Hiroshi Hatanaka, Toshiro Ozawa, Tsuneo Hashi

Published Jun 1, 1977• 21 citations
Publisher

Abstract

Two-quantum rotary echoes predicted by Bloch like equations for two-quantum transition have been observed in a multi-level NMR system of 27 Al nuclei in Al 2 O 3 . An rf field exactly at resonance to the two-quantum transition ( Δ m =2) was turned on at t =0 and its phase was shifted by 90° at t =τ. The echo at t =2τ was observed by using the technique of transfer of coherence reported previously. Characteristic dependence of the echo width upon inhomogeneity of rf field amplitude was confirmed experimentally.

DOI
10.1143/jpsj.42.2069

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Large-amplitude oscillations are predicted in the free-induction decay (FID) of atomic or spin two-level quantum systems that are coherently prepared by a resonant electromagnetic field in the form of a square amplitude pulse of duration $T$. The effect should be detectable in nuclear magnetic resonance (NMR) or in optical resonance experiments when the transition line shape is inhomogeneously broadened (${T}_{2}^{*}\ensuremath{\ll}{T}_{2}$) and the applied field is intense enough that the pulse area $\ensuremath{\chi}T\ensuremath{\ge}2\ensuremath{\pi}$, where $\ensuremath{\chi}$ is the Rabi frequency. Physically, the effect is due to Rabi oscillations which are generated in the preparative stage and are then reproduced because of atomic memory in the radiative period which follows. The atomic polarization derived from the Bloch equations assumes the form of an integral over the inhomogeneous line shape, and can be evaluated numerically for arbitrary linewidth $\ensuremath{\sigma}$ or analytically when $\ensuremath{\sigma}\ensuremath{\rightarrow}\ensuremath{\infty}$. The characteristics of the oscillation are unusual since the oscillation frequency, which is of order $\ensuremath{\chi}$, increases with time while the oscillation envelope vanishes identically for times $t\ensuremath{\ge}2T$. Coherent emission is therefore confined to one pulse width $T$ immediately following the pulse. Previous NMR and infrared FID experiments with small-area pulses ($\ensuremath{\chi}T\ensuremath{\le}4\ensuremath{\pi}$), interpreted erroneously in terms of an edge echo effect, support the oscillatory FID behavior described here. For the case $\ensuremath{\chi}T>4\ensuremath{\pi}$, an experimental test would be even more decisive, as the oscillations are more pronounced.

Physical Review A•Mar 1, 1980•57 citations
Two-quantum rotary echoes predicted by Bloch like equations for two-quantum transition have been observed in a multi-level NMR system of 27 Al nuclei in Al 2 O 3 . An rf field exactly at resonance to the two-quantum transition ( Δ m =2) was turned on at t =0 and its phase was shifted by 90° at t =τ. The echo at t =2τ was observed by using the technique of transfer of coherence reported previously. Characteristic dependence of the echo width upon inhomogeneity of rf field amplitude was confirmed experimentally.
The first observation of optical rotary echoes, the optical analog of rotary spin echoes, is reported. Rotary echoes are produced in a quantum-mechanical two-level system which is driven resonantly (nutation effect) by a coherent field that suffers a sudden phase retardation. The initial nutation transient dephases, because of an inhomogeneity in either the driving field or the transition frequency of the sample, and then rephases to form an echo following the phase-shifting pulse. Hence, optical rotary and photon echoes are similar processes---the former being an interference in nutation and the latter an interference in free precession. Perturbative solutions of the Bloch equations are derived for the case where inhomogeneous dephasing arises from Doppler broadening and the Rabi frequency exceeds the homogeneous damping rate. Observations of the optical rotary echo in I2{\mathrm{I}}_{2}I2​ vapor are facilitated by the technique of laser frequency switching, which generates precise phase shifts in the optical field. The measurements corroborate detailed theoretical predictions.
The phenomenon of transfer of coherence and the effect of level shift caused by two-quantum (TQ) excitation were studied on 27Al^{27}\mathrm{Al}27Al nuclei in Al2{\mathrm{Al}}_{2}Al2​O3{\mathrm{O}}_{3}O3​. Transfer of coherence between two single-quantum (SQ) transitions and that between SQ and three-quantum transitions were examined. It was observed that the coherences transfer periodically with frequency equal to one-half the TQ transient nutation frequency accompanied by phase shifts caused by the level shift. Experimental results are in good agreement with theoretical predictions. The effect of magnetic dipole interaction was also studied. A precise measurement was made on the shift of TQ resonance frequency and it was confirmed that no shift exists on the TQ resonance frequency contrary to the prediction based on the three-level model.
We present a theory of optical two-photon rotary echo for the case when the direct couplings between the three levels due to spontaneous decay to and from the intermediate state dominate the indirect couplings (collisional, etc.) to the passive levels and the phase-interrupting (P.I.) collisions cannot be ignored. For this situation which generally obtains in the visible/U.V. region which is relevant for many two-photon transient experiments, the ‘two-photon Bloch equations’ with non-resonant intermediate state are non-trivially different from the familiar (two-level) Bloch equations with or without direct coupling. An explicit analytical calculation demonstrates two-photon rotary echo with the usual dependence on the total phase shift. The dependence of the echo peak on pulse delay time is governed by a damping constant in which ‘intensity modification’ involves only the P.I. collision constant and not the spontaneous decay constant in sharp contrast to the one-photon case. For the case of counter-propagating beams, the intensity modified echo damping constant turns out to be especially simple. We suggest that the features unique to the two-photon rotary echo can be usefully exploited for the empirical determination of the polarization decay constant.
A general expression for coherent transients, free induction decay and echoes, of an atomic or spin two-level system excited by resonant laser or rf field in the form of two square pulses is given by using the Fourier-transform method. This expression interprets the main characteristics of the transient signals well. An analytic expression for the shapes of two-pulse echoes is derived by assuming infinite inhomogeneity and the same Rabi frequencies for the two pulses. Two-pulse echo shapes were numerically calculated for various combinations of pulse areas by using the analytic expression. Nuclear-magnetic-resonance experiment was carried out on an inhomogeneously broadened proton spin system. Experimental two-pulse echo shapes are compared with the calculated ones. Agreement between theory and experiment is quite excellent.
Large-amplitude oscillations are predicted in the free-induction decay (FID) of atomic or spin two-level quantum systems that are coherently prepared by a resonant electromagnetic field in the form of a square amplitude pulse of duration TTT. The effect should be detectable in nuclear magnetic resonance (NMR) or in optical resonance experiments when the transition line shape is inhomogeneously broadened (${T}_{2}^{*}\ensuremath{\ll}{T}_{2}$) and the applied field is intense enough that the pulse area $\ensuremath{\chi}T\ensuremath{\ge}2\ensuremath{\pi}$, where $\ensuremath{\chi}$ is the Rabi frequency. Physically, the effect is due to Rabi oscillations which are generated in the preparative stage and are then reproduced because of atomic memory in the radiative period which follows. The atomic polarization derived from the Bloch equations assumes the form of an integral over the inhomogeneous line shape, and can be evaluated numerically for arbitrary linewidth $\ensuremath{\sigma}$ or analytically when $\ensuremath{\sigma}\ensuremath{\rightarrow}\ensuremath{\infty}$. The characteristics of the oscillation are unusual since the oscillation frequency, which is of order $\ensuremath{\chi}$, increases with time while the oscillation envelope vanishes identically for times $t\ensuremath{\ge}2T$. Coherent emission is therefore confined to one pulse width TTT immediately following the pulse. Previous NMR and infrared FID experiments with small-area pulses ($\ensuremath{\chi}T\ensuremath{\le}4\ensuremath{\pi}$), interpreted erroneously in terms of an edge echo effect, support the oscillatory FID behavior described here. For the case $\ensuremath{\chi}T>4\ensuremath{\pi}$, an experimental test would be even more decisive, as the oscillations are more pronounced.